文献类型：期刊文献

英文题名：Single-atomic-site iron on N-doped carbon for chemoselective reduction of nitroarenes

作者：Lu, Guoping[1] Sun, Kangkang[1] Lin, Yamei[3] Du, Qixuan[1] Zhang, Jiawei[4] Wang, Kui[2] Wang, Pengcheng[1]

第一作者：Lu, Guoping

通信作者：Wang, PC[1];Wang, K[2]

机构：[1]Nanjing Univ Sci & Technol, Sch Chem Engn, Nanjing 210094, Peoples R China;[2]Chinese Acad Forestry, Natl Engn Lab Biomass Chem Utilizat, Inst Chem Ind Forest Prod, Nanjing 210042, Peoples R China;[3]Nanjing Normal Univ, Sch Food Sci & Pharmaceut Engn, Nanjing 210032, Peoples R China;[4]Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Peoples R China

年份：2022

卷号：15

期号：1

起止页码：603-611

外文期刊名：NANO RESEARCH

收录：;EI(收录号：20213110703940);Scopus(收录号：2-s2.0-85110472510);WOS:【SCI-EXPANDED(收录号:WOS:000678460700006)】；

基金：We gratefully acknowledge the Fundamental Research Funds for the Central Universities (No. 30920021120), the Key Laboratory of Biomass Energy and Material, Jiangsu Province (No. JSBEM201912), the National Natural Science Foundation of China (No. 21905089), and the Chinese Postdoctoral Science Foundation (No. 2019M662775) for financial support.

语种：英文

外文关键词：single-atom-site iron; zeolitic imidazolate framework; the hydrogenation of nitroarene; N-doped carbon; drug synthesis

摘要：A facile, gram-scale and sustainable approach has been established for the synthesis of single-atomic-site iron on N-doped carbon (Fe-SA@NC-20A) via the pyrolysis of aniline modified FeZn-ZIFs, in which the synthesis of zeolitic imidazolate frameworks (ZIFs) can be accomplished in water at room temperature, and no acid etching is required. The as-synthesized catalyst exhibits better performance on the chemoselective hydrogenation of nitroarenes with a broad substrate scope (turnover frequency (TOF) up to 1,727 h(-1), 23 examples) than most of previously reported works. Based on high-angle annular dark field scanning transmission microscopy (HAADF-STEM) images in combination with X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), electron spin resonance (ESR), and Mossbauer spectroscopy, Fe is dispersed as single atoms via forming FeNx (x = 4-6). This work not only determines the active sites of Fe-SA@NC-20A for hydrogenation (FeN4), but also proposes tentative pathways for both N-H activation of hydrazine and the reduction of nitroarene on FeN4 site, both of which are the key steps for the hydrogenation of nitroarenes. In addition, this catalyst shows excellent stability, and no significant activity degradation is observed when recycling for 10 times or restoring in air for 2 months.